Dual-atom catalysts (DACs) have gained great attention as highly efficient materials for the hydrogen evolution reaction (HER) due to their synergistic dual-site effects and high atomic utilization. This review explores how microenvironmental regulation, including electronic structure optimization and coordination design, influences DAC performance. Both homonuclear and heteronuclear types of DACs are analyzed in detail in terms of their site interactions and structural configurations. Moreover, recent advancements of DACs in HER applications under various pH conditions are discussed, highlighting their enhanced catalytic activity and mechanism. Despite challenges in synthesis and characterization, DACs represent a promising frontier for developing efficient HER catalysts and offer guidance for future research and scalable applications.

Nitride family compounds are among the earliest explored materials for solid electrolytes (SEs). The main challenge lies in effectively enhancing their electrochemical stability without compromising their excellent Li-ion conductivity and Li metal compatibility. Herein, a H delta --H delta + comproportionation reaction between LiH and NH4F is employed to synthesize a Li-N-H-F complex, consisting of Li2+ xNHFx matrix and dispersed LiF nanoparticles. Density functional calculation results show that the incorporated F atoms in Li2NH lattice lead to structural variation and electron density redistribution, providing a more connected Li-ion network with low migration energy barriers. More importantly, the interfacial side reactions between the Li-N-H-F complex and electrodes are strongly self-limited due to the blocking effect of the in situ formed Li4NH/LiF-enriched interphases. The newly identified interphase Li4NH exhibits fast Li-ion migration ability and intrinsic stability toward Li, facilitating stable Li plating/stripping. Based on the superiority in Li-ion conduction and electrode compatibility, the Li-N-H-F solid electrolyte films prepared via cold pressing with 0.5 wt% binder enable stable cycling of Li||Li, Li||TiS2, and Li||LiCoO2 all-solid-state batteries.

Rechargeable magnesium batteries (RMBs) are regarded as one of the most promising candidates for next-generation battery technologies. However, their practical implementation remains significantly hindered due to the lack of suitable non-nucleophilic electrolytes and the persistent challenge of Mg anode passivation. Herein, we engineered a halogen-enhanced Mg(AlCl4)(2)-IL-DME-M4-I-2 electrolyte by strategically incorporating 50 mM iodine additives into the Mg(AlCl4)(2)-IL-DME-M4 system, achieving robust Mg plating/stripping reversibility, low overpotential and enhanced anodic stability. The enhanced electrochemical performance arouse mainly from the in-situ formed dual-conductive MgF2/MgI2 interfacial layer, which effectively prevented Mg anode passivation and suppressed parasitic electrolyte decomposition. The Mg/S battery system employing the Mg(AlCl4)(2)-IL-DME-M4-I-2 electrolyte and MoS2@CMK/S composite cathode demonstrated exceptional electrochemical performance, delivering a record reversible capacity of 1541 mAh g(-1) at 0.1C, coupled with exceptional rate capability and sustained cycling stability (348 mAh g(-1) retention over 600 cycles at 0.5C) while maintaining similar to 100 % coulombic efficiency. This work establishes a promising and feasible strategy for developing high-efficiency non-nucleophilic magnesium electrolytes.

The cycle life of aqueous zinc batteries is hindered by undesired side reactions and dendrite growth of the Zn metal anode due to the lack of an advanced solid electrolyte interphase. Here, a pioneering self-assembled electrode-electrolyte interphase (AEEI) constructed from electrolyte additives of amphiphilic molecules (APMs) is presented. Specifically, polyvinyl pyrrolidone (PVP) molecules are demonstrated due to their high electron-donating property of the carbonyl oxygen atoms in pyrrolidone groups that conjugate with aromatic pyrrole rings. The formation and stability of this interphase is fundamentally prompted by the interaction between the carbonyl oxygen atoms of APMs and Zn metal as well as Zn2+ ions, which is elucidated by X-ray photoelectron spectroscopy and Fourier transform infrared spectroscopy. The resultant AEEI predominantly consists of a dense lamellar micelle of APMs enriched with Zn2+ ions. Maintaining the contents of APMs above a critical aggregation concentration of ∼0.1

High-entropy perovskite ceramics have garnered widespread attention in the energy storage field due to their diversified composition and superior performance. However, the preparation of high-performance high-entropy ceramic materials still faces many challenges due to their complex composition and structure. This work systematically studies the effects of MgO, SiO2, Li2CO3, and MnCO3 on the sintering temperature and energy storage performance of (Na0.2Bi0.2Ba0.2Sr0.2Ca0.2)TiO3 (NBBSCT) high-entropy ceramics. The introduction of MnCO3 successfully reduced the sintering temperature of the high-entropy ceramics to 1150 degrees C and achieved a high energy storage efficiency of 95.5% with this composition. The NBBSCT ceramics with 0.5 wt%MgO exhibited a breakdown field of 300 kV/cm and an energy storage density of 3.7 J/cm3. The study indicates that adding appropriate sintering aids can significantly improve the sintering behavior and energy storage performance of high-entropy ceramics. This method provides new insights into the preparation and performance enhancement of high-entropy energy storage ceramics.

High-entropy ceramics, as a newly discovered type of material in recent years, have attracted widespread attention due to their unique structure and high-entropy effects. However, due to the sluggish diffusion effects inherent in high entropy, these ceramics require prolonged sintering at high temperatures to achieve full densification, leading to long fabrication cycles and significant energy consumption. This study utilized flash sintering to successfully obtain dense single-phase high-entropy ceramics in just 60 s while lowering the furnace temperature by 400 degrees C. Various tests demonstrate that the application of an external electric field during flash sintering promotes material diffusion and densification processes, effectively suppressing excessive grain growth and elemental volatilization. Consequently, the high-entropy ceramics (Na 0.2 Bi 0.2 Ba 0.2 Sr 0.2 Ca 0.2 )TiO 3 exhibit outstanding energy storage performance ( W rec = 5.8 J/cm3) 3 ) under moderate electric fields. This research confirms the feasibility of flash sintering in the preparation of dielectric materials for capacitors, providing a practical and cost-effective approach for the low-cost and sustainable development of the ceramic manufacturing industry.

The exploration and development of efficient and cost-effective oxygen reduction reaction (ORR) catalysts for non-metallic biomass have emerged as a crucial avenue for synthesizing diverse carbon nanomaterials.

Platinum-based catalysts are considered the most effective catalysts for the hydrogen evolution reaction (HER) in acidic media; however, they exhibit poor performance in alkaline electrolysis waters, which are currently more commercially developed, due to their sluggish water dissociation ability. Small-sized metal Ru nanoparticles, with metal-hydrogen bond strength close to Pt (approximately 65 kcal/mol) and a relatively lower water dissociation barrier, are considered one of the most promising alternatives to the noble metal Pt for alkaline HER. Based on the above statements, the present study innovatively combines the effective strategies of "heterogeneous interface engineering" and "construction of ultrafine active sites" to develop a highly efficient Ru-based catalyst with a three-phase heterogeneous interface, aiming to form its application in alkaline HER. Characterization analysis and DFT calculations demonstrated that the "Rux-Ni(OH)(2)-NiO" three-phase heterogeneous interface constructed around ultrafine Rux clusters effectively modulated the electronic structure of the overall material and optimized the HER kinetic steps. This catalytic material, Rux@NOH/NO, exhibited outstanding electrocatalytic activity in alkaline HER, requiring only 44.2 mV to drive a current density of 10 mA center dot cm(-2), with excellent long-term stability and extremely low active material loading (1.36 wt%-Ru). Specially, its mass activity reached an impressive 18,897.1 A/gRu at 150 mV, which is 10.2 times higher than that of commercial 20wt % Pt/C. In summary, this study synergistically constructs an ultrafine metal ruthenium-based catalyst based on a three-phase heterogeneous interface using a composite strategy, which provides an effective catalyst system for alkaline HER catalytic reactions and holds significance for the rational construction and design of efficient heterogeneous interface electrocatalysts.

Photothermal energy has been widely used in high-tech applications, such as heating/cooling systems, bio-imaging, bio-sensing, and medical therapies. However, conventional photothermal materials have narrow photo-absorption bandwidth and low photothermal conversion efficiency. Innovative materials that can more efficiently harvest photothermal energy are highly demanded. Topological insulator materials with excellent optical properties hold great potential in photo-absorption and photothermal conversion. This work investigated and engineered photo-absorption and photothermal effect in Sb2Te3 topological insulator nanograting. The TI material was grown by metal-organic chemical vapor deposition to exploit the benefits of the process, yielding high material quality and large deposition areas. Through a meticulous process encompassing material synthesis, engineering, and characterization, highly absorptive Sb2Te3 topological insulator nanograting and efficient photothermal conversion have been achieved. This research contributes to the advancement of the fundamental knowledge of light–matter interaction and photothermal effects in topological insulator materials. The outcomes of this study can benefit the development of efficient photothermal materials for high-performance nano-energy and biomedical technologies.

The poor electrochemical reaction kinetics of Li polysulfides is a key barrier that prevents the Li-S batteries from widespread applications. Ni single atoms dispersed on carbon matrixes derived from ZIF-8 are a promising type of catalyst for accelerating the conversion of active sulfur species. However, Ni favors a square-planar coordination that can only be doped on the external surface of ZIF-8, leading to a low loading amount of Ni single atoms after pyrolysis. Herein, we demonstrate an in situ trapping strategy to synthesize Ni and melamine-codoped ZIF-8 precursor (Ni-ZIF-8-MA) by simultaneously introducing melamine and Ni during the synthesis of ZIF-8, which can remarkably decrease the particle size of ZIF-8 and further anchor Ni via Ni-N6 coordination. Consequently, a novel high-loading Ni single-atom (3.3 wt %) catalyst implanted in an N-doped nanocarbon matrix (Ni@NNC) is obtained after high-temperature pyrolysis. This catalyst as a separator modifier shows a superior catalytic effect on the electrochemical transitions of Li polysulfides, which endows the corresponding Li-S batteries with a high specific capacity of 1232.4 mA h g-1 at 0.3 C and an excellent rate capability of 814.9 mA h g-1 at 3 C. Furthermore, a superior areal capacity of 4.6 mA h cm-2 with stable cycling over 160 cycles can be achieved under a critical condition with a low electrolyte/sulfur ratio (8.4 μL mg-1) and high sulfur loading (4.85 mg cm-2). The outstanding electrochemical performances can be attributed to the strong adsorption and fast conversion of Li polysulfides on the highly dense active sites of Ni@NNC. This intriguing work provides new inspirations for designing high-loading single-atom catalysts applied in Li-S batteries.

Hydrogen (H2) production from alkaline water electrocatalysis is economically appealing yet significantly hindered by the sluggish H2O adsorption and H* binding kinetics on active sites during hydrogen evolution reaction (HER). Herein, we interfacially immobilize Ru clusters on the hierarchical nickel nitride (Ru-Ni3N) nanosheet arrays via the filling of Ru3+ species into the metal vacancies of nickel hydroxide precursors and the subsequent controllable nitridation. The optimized Ru-Ni3N shows the outstanding HER performance, affording a 30-fold rise in the intrinsic activity of Ni sites, a outperforming-Pt/C overpotential at ≥125 mA cm-2 while remaining a robust stability. We further establish by a combined study of density functional theory (DFT) calculations with experimental analyses that long-range Ni sites around Ru sites act as active sites via the electron delocalization, remarkably weakening the H2O adsorption and H* binding barriers for enhancing the alkaline HER kinetics. Moreover, it also demonstrates an excellent pH-universal HER and overall water splitting performance.

Single-atom catalysts, featuring some of the most unique activities, selectivity, and high metal utilization, have been extensively studied over the past decade. Given their high activity, selectivity, especially towards small molecules or key intermediate conversions, they can be synergized together with other active species (typically other single atoms, atomic clusters, or nanoparticles) in either tandem or parallel or both, leading to much better performance in complex catalytic processes. Although there have been reports on effectively combining the multiple components into one single catalytic entity, the combination and synergy between single atoms and other active species have not been reviewed and examined in a systematic manner. Herein, in this overview, the key synergistic interactions, binary complementary effects, and the bifunctional functions of single atoms with other active species are defined and discussed in detail. The integration functions of their marriages are investigated with particular emphasis on the homogeneous and heterogeneous combinations, spatial distribution, synthetic strategies, and the thus-derived outstanding catalytic performance, together with new light shined on the catalytic mechanisms by zooming in several case studies. The dynamic nature of each of the active species and in particular their interactions in such new catalytic entities in the heterogeneous electrocatalytic processes are visited, on the basis of the in situ/operando evidence. Last, we feature the current challenges and future perspectives of these integrated catalytic entities that can offer guidance for advanced catalyst design by the rational combination and synergy of binary or multiple active species.

Electrochemical carbon dioxide (CO2) reduction (ECR) is a commercially promising technology to resolve the energy dilemma and accomplish carbon recycling. Herein, a novel electrocatalyst is dedicated to producing HCOOH during ECR process by tuning the interfacial interaction via loading SnO2@C on Cu2S. The snowflake Cu2S with loading 1 wt. % SnO2@C shows a Faradaic efficiency of HCOOH as high as 88% at -1.0 V versus reversible hydrogen electrode in comparison to pure Cu2S and a stable current density of 15.6 mA cm -2 . Combined investigations using in-situ infrared spectra with in-situ Raman spectra reveal that the active species is Cu+ . And the Cu2S/1%SnO2 @C can effectively promote the adsorption and activation of carbonate and inhibit the production of CO intermediates. The corresponding density functional theory (DFT) demonstrates that the Cu2S/1%SnO2@C can well stabilize the *OCHO intermediate during ECR process. The interaction between the Cu2S and SnO2 @C adjusts the surface electronic distributions and accelerates electron transfer, which facilitates the HCOOH selectivity of ECR. The result obtained from this work provides a simple and efficient electrocatalyst towards HCOOH production by ECR with improving efficiency and selectivity.

Diseases caused by flaviviruses such as dengue virus (DENV) and West Nile Virus (WNV), are a serious threat to public health. The flavivirus single-stranded RNA genome is translated into a polyprotein which is cleaved into three structural proteins and seven non-structural proteins by the viral and cellular proteases. Non-structural (NS) protein 3 is a multifunctional protein that has N-terminal protease and C-terminal helicase domains. The NS3 protease requires co-factor NS2B for enzymatic activity and folding. Due to its essential role in viral replication, NS2B-NS3 protease is an attractive target for antiviral drugs. Despite the availability of crystal structures, dynamic interactions of the N- and C-termini of NS2B co-factor have been elusive due to their flexible fold. In this study, we employ integrative structural approaches combined with biochemical assays to elucidate the dynamic interactions of the flexible DENV4 NS2B and NS3 N- and C-termini. We captured the crystal structure of self-cleaved DENV4 NS2B47NS3 protease in post cleavage state. The intermediate conformation adopted in the reported structure can be targeted by allosteric inhibitors. Comparison of our new findings from DENV4 against previously studied ZIKV NS2B-NS3 proteins reveals differences in NS2B-NS3 function between the two viruses. No inhibition of protease activity was observed for unlinked DENV NS2B-NS3 in presence of the cleavage site while ZIKV NS2B-NS3 cleavage inhibits protease activity. Another difference is that binding of the NS2B C-terminus to DENV4 eNS2B47NS3Pro active site is mediated via interactions with P4-P6 residues while for ZIKV, the binding of NS2B C-terminus to active site is mediated by P1-P3 residues. The mapping of NS2B N- and C-termini with NS3 indicates that these intermolecular interactions occur mainly on the beta-barrel 2 of the NS3 protease domain. Our integrative approach enables a comprehensive understanding of the folding and dynamic interactions of DENV NS3 protease and its cofactor NS2B.

Electrochemical carbon dioxide reduction (ECR) is an attractive pathway to synthesize useful fuels and chemical feedstocks, especially when paired with renewable electricity as the energy source. In this overview, we examine the recently witnessed advances and on-going pursuits of ECR in terms of the key fundamental mechanisms, basic experimentation principles, electrocatalysts and the electrochemical setup for ECR, aiming at offering timely key insights into solving the unsettled bottleneck issues. The reaction pathways are discussed in relation to the generation of single-, double- and multi-carbon products by the ECR, as well as the underlying principles in catalyst design to form them both efficiently and selectively. For the rational design of electrocatalysis, we look into the critically important roles played by various in situ and operando experimental techniques and computational simulations, where the key priorities are to engineer the highly active and selective ECR catalysts for the specifically targeted products. Indeed, with the purposely designed high activity and selectivity, one would be able to “magically” transform a bottle of CO2-riched “coke drink” to a glass of “beer” with the desired alcohol product in a layman term, instead of a bottle of formic acid. Nonetheless, there are still considerable complications and challenges ahead. As a dynamically rapid-advancing research frontier for both energy and the environment, there are great opportunities and obstacles in the ECR scale up. Electrochemical CO2 reduction, where the “spirit” is brewing on electrocatalytic activity and selectivity. With the designed catalytic activity and selectivity, one would be able to magically transform a bottle of CO2-riched “coke” into a glass of “beer”.

Electrocatalytic oxygen evolution reaction (OER) is a crucial anode reaction where electrocatalysts are the key elements and their dynamic surface chemistry runs throughout the entire process. Herein, we examine the latest advances and challenges in understanding of the dynamic surface chemistry of OER electrocatalysts. There are electrochemical origin and driving force for the dynamic surface nature, where several processes can take place either concurrently or sequentially, including reconstruction (i.e., phase formation/transformation, morphological change, and compositional change), vacancy generation and filling/refilling, and the intermediate adsorption–desorption process on catalytic surface. These dynamic surface processes of OER catalysts are impacted by not only the reaction and service conditions, including the (local) pH and its gradient distribution, applied potential, types and concentration of exotic ions and external fields on top of the nature of catalysts/precatalysts, but also their interactions. Due to the local, time‐dependent and instant nature, there are considerable challenges in tracing, modelling and understanding of the complete dynamic surface chemistry of catalysts in OER, by means of ex situ, in situ and operando experimental investigations. Therefore, computational studies and dynamic simulations help provide key insights in future pursuits, where there is critical need for a multiscale computational modelling approach encompassing all these aspects.

The development of 1D fiber‐shaped supercapacitors (SCs) with high volumetric energy density is of great significance for miniature wearable electronics, where limiting the device's volume is critical. In this study, a partially unzipped carbon nanotube/reduction graphene oxide (PUCNT/RGO) hybrid fiber with less “dead volume” and a well‐ordered porous structure is fabricated via wet spinning of a mixed partially unzipped oxidized carbon nanotube (PUOCNT)/GO solution and chemical reduction. The spinning solution is of low viscosity and high concentration, which can ensure smooth spinning while reducing the mass transfer during phase separation, thus lessen the “dead volume” derived from isolated pores. Moreover, PUOCNT with 1D and 2D hybrid nanoarchitecture, large specific surface area, and good water solubility can be a more effective spacer to inhibit the restacking of graphene oxide sheets while reducing the spacer itself and the large spacious voids formed “dead volume”. The all‐solid‐state SC assembled from the PUCNT/RGO hybrid fiber exhibits an excellent volumetric energy density of 8.63 mWh cm −3 , exceeding the values of previously reported carbon‐based fibers. The findings may open a door for finely controlling the density and pore structure of graphene‐based fiber for applications in high volumetric energy storage via a scalable and efficient process.

The concept of single atom catalysts (SACs) originated from reducing the amount of noble metals used, by steadily refining the particle size loaded on a substrate surface. It has been rapidly moving to non-noble elements and their compounds in recent years, notably transition metals and even non-metals. They are of heterogeneous types, where the active species are refined to atomic dispersion scales on the surfaces/sub-surfaces of the solid support. The catalytic performance is governed by both the type and population of accessible active sites, and their bond and coordination environment, largely as a result of the interactions with the substrate surface. Unlike the internal structure within a crystalline solid, there is a large spatial variation in the bond and coordination environment of different atoms on the solid surface across different length scales, and in particular with the unsaturated surface, where there are various defects. They can also be dramatically altered during both the catalyst synthesis and actual catalysis process. In a way, they form a "surface heterocompound", where the local bonds for each metal atom are of a compound type, while there can be a large variation from one to another. Herein, we will look into the evolution from traditional heterogeneous catalysts to SACs, from the surface heterocompound perspective. Discussion will then be made on the on-going strategies and challenges in manipulating and identifying the local bond and coordination environment on the hetero-surfaces, in an attempt to develop efficient catalysts for the targeted applications, where both synthesis techniques and analytical tools are critically important, and computational studies can provide the key guiding principles. With selected paradigm studies, we will briefly examine the future perspectives for this newly emerging catalysis frontier.